Oligoyne bridges enable strong through-bond coupling and efficient triplet transfer from CdSe QD trap excitons for photon upconversion.

Polyyne bridges have attracted extensive interest as molecular wires due to their shallow distance dependence during charge transfer. Here, we investigate whether triplet energy transfer from cadmium selenide (CdSe) quantum dots (QDs) to anthracene acceptors benefits from the high conductance associated with polyyne bridges, especially from the potential cumulene character in their excited states. Introducing π-electron rich oligoyne bridges between the surface-bound anthracene-based transmitter ligands, we explore the triplet energy transfer rate between the CdSe QDs and anthracene core.

High-Level Reverse Intersystem Crossing and Molecular Rigidity Improve Spin Statistics for Triplet-Triplet Annihilation Upconversion.

The structural factors affecting triplet-triplet annihilation (TTA) at the molecular level are not well-understood. Here, our steady-state photoluminescence and transient absorption results demonstrate that the spin statistical factor, η, decreases from 0.60 to 0.

On the size-dependence of CdSe nanocrystals for photon upconversion with anthracene.

In triplet-triplet annihilation based photon upconversion, controlling triplet energy transfer (TET) through the system is key to unlocking higher efficiencies. In this work, we vary the size of colloidally synthesized CdSe nanocrystals (NCs) to examine the effects on TET during photon upconversion, using steady-state measurements and transient absorption spectroscopy. As the CdSe NC size increases, the photon upconversion quantum yield (QY) decreases due to the decrease in the rate of TET from CdSe to the surface bound anthracene transmitter ligand, as expected for the Marcus description of energy transfer from the transmitter to the NC.

Enhanced Near-Infrared-to-Visible Upconversion by Synthetic Control of PbS Nanocrystal Triplet Photosensitizers.

Photon upconversion employing semiconductor nanocrystals (NCs) makes use of their large and tunable absorption to harvest light in the near-infrared (NIR) wavelengths as well as their small gap between singlet and triplet excited states to reduce energy losses. Here, we report the highest QY (11.8%) thus far for the conversion of NIR to yellow photons by improving the quality of the PbS NC.